AbstractThe <110>‐oriented BaTiO3 ceramics were fabricated using BaCO3 matrix and H1.08Ti1.73O4.nH2O (HTO) template particles, and the mechanism of BaTiO3 phase formation was investigated. The dielectric, ferroelectric, and piezoelectric properties were also investigated. The transformation of the HTO phase into the TiO2 bronze or TiO2 (B) phase was observed at 600°C, where the BaTiO3 nucleation was accompanied by the formation of a Ba2TiO4 phase. The TiO2 phase reacted with the Ba2TiO4 phase at 800°C to give a BaTiO3 phase, whereas its reaction with the BaTiO3 resulted in the formation of BaTi2O5 phase that got decomposed into BaTiO3 and Ba6Ti17O40 phase at sintering temperature ≥1300°C. Sintering with samples’ embedding in BaTiO3 powders prevented the formation of the Ba6Ti17O40 secondary phase. The crystallographic orientation along the <110> direction (F110) was developed by the epitaxial grain growth mechanism. In addition to the contribution of the grain‐size increment for enhancing the F110, the preservation of the platelike structure was also found to have a significant impact. The ceramics prepared by the embedded sintering (grain size ≈12.4 µm and F110 = 83%) exhibited the room‐temperature dielectric constant of 1708 and piezoelectric strain constant of 445 pm/V, which are higher than those of the BaTiO3 ceramics with randomly oriented grains.